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Tuning the Mechanical Properties of 3D-printed Objects by the RAFT Process: From Chain-Growth to Step-Growth

Angewandte Chemie 2024年第10期136卷

作者： Xiaofeng Pan Dr. Jiajia Li Zhuang Li Qing Li Dr. Xiangqiang Pan Zhengbiao Zhang Prof. Jian Zhu State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and Engineering College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China

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A Novel Side-Chain Liquid Crystal Elastomer Exhibiting Anomalous Reversible Shape Change

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Angewandte Chemie 2020年第35期132卷 15241-15246页

作者： Yin L. Han L. Ge F. Tong X. Zhang W. Soldera A. Zhao Y. Département de chimie Université de Sherbrooke Sherbrooke QC J1K 2R1 Canada Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou Industrial Park Suzhou 215123 China

Liquid crystalline elastomers (LCEs) have been actively investigated as stimuli-controlled actuators and soft robots. The basis of these applications is the ability of LCEs to undergo a reversible shape change upon a liquid crystalline (LC)-isotropic phase transition. Herein, we report the synthesis of a novel LCE based on a side-chain liquid crystalline polymer (SCLCP). In contrast to known LCEs, this LCE exhibits a striking anomalous shape change. Subjecting a mechanically stretched monodomain strip to LC-disorder phase transition, both the length and width of the strip contract in isotropic phase, and both elongate in LC phase. This thermally induced behaviour is the result of a subtle interplay between the relaxation of polymer main chain oriented along the stretching direction and the disordering of side-group mesogens oriented perpendicularly to the stretching direction. This finding points out potential design of LCEs of this peculiar type and possible applications to exploit. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

关键词： auxetic-like shape change liquid crystal elastomer reversible shape memory soft actuator

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Ultra-Fast Selenol-Yne Click (SYC) Reaction Enables Poly(selenoacetal) Covalent Adaptable Network Formation

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Angewandte Chemie 2024年第40期136卷

作者： Mengyao Zhang Sisi Chen Guichuan Xu Weihong Lu Jiajia Li Jiandong Zhang Zhengbiao Zhang Jian Zhu Xiangqiang Pan State and Local Joint Engineering Laboratory for Novel Functional Department Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and Engineering College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China

The emergence of covalent adaptable networks (CANs) based on dynamic covalent bonds (DCBs) presents a promising avenue for achieving resource recovery and utilization. In this study, we discovered a dynamic covalent bond called selenacetal, which is obtained through a double click reaction between selenol and activated alkynes. Density functional theory (DFT) calculations demonstrated that the ΔG for the formation of selenoacetals ranges from 12 to 18 kJ mol −1 , suggesting its potential for dynamic reversibility. Dynamic exchange experiments involving small molecules and polymers provide substantial evidence supporting the dynamic exchange properties of selenoacetals. By utilizing this highly efficient click reaction, we successfully synthesized dynamic materials based on selenoacetal with remarkable reprocessing capabilities without any catalysts. These materials exhibit chemical recycling under alkaline conditions, wherein selenoacetal (SA) can decompose into active enone selenide (ES) and diselenides. Reintroducing selenol initiates a renewed reaction with the enone selenide, facilitating material recycling and yielding a newly developed dynamic material exhibiting both photo- and thermal responsiveness. The results underscore the potential of selenoacetal polymers in terms of recyclability and selective degradation, making them a valuable addition to conventional covalent adaptable networks.

关键词： Covalent Adaptable Networks Dynamic Covalent Chemistry Click Reaction Selenoacetal

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Redox-responsive ferrocene-containing poly(ionic liquid)s for antibacterial applications

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Science China Chemistry 2019年第1期62卷 95-104页

作者： Tikai Zhang Jiangna Guo Yingying Ding Hailei Mao Feng Yan Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and EngineeringCollege of Chemistry Chemical Engineering and Materials Science Soochow University Department of Anesthesiology and Critical Care Medicine Zhongshan Hospital Fudan University

Ferrocene(Fc)-containing imidazolium type ionic liquids(ILs) and corresponding poly(ionic liquid)(PIL) membranes with tunable antibacterial activity based on electrochemical redox reaction and host-guest chemistry were developed. The effect of Fc moiety on the antimicrobial activities against both Staphylococcus aureus(S. aureus) and Escherichia coli(E. coli) was studied by minimum inhibitory concentration(MIC). The presence of Fc groups highly enhanced the antibacterial efficiency of Fccontaining ILs because of the generation of reactive oxygen species(ROS). The electrochemical oxidation of Fc to Fc+and the formation of inclusion complexes between Fc and β-CD via host-guest interactions decreased the antibacterial activities of ILs and PIL membranes. The antibacterial activities may be recovered in some extent upon the electrochemical reduction of Fc+to Fc or the exclusion of the Fc out of the cavity of β-CD. Furthermore, all the Fc-containing PIL membranes showed relatively low hemolysis activities and none cytotoxicity toward human cells, indicating clinical feasibility in topical applications.

关键词： antibacterial activities imidazolium cations ferrocene poly(ionic liquid) cytotoxicity

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Intrinsic and extrinsic anomalous transport properties in noncollinear antiferromagnetic Mn3Sn from first-principle calculations

arXiv

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arXiv 2023年

作者： Yang, Xiuxian Feng, Wanxiang Zhou, Xiaodong Mokrousov, Yuriy Yao, Yugui Beijing Key Lab of Nanophotonics & Ultrafine Optoelectronic Systems School of Physics Beijing Institute of Technology Beijing100081 China School of Physics Jiangsu Normal University Xuzhou221116 China Laboratory of Quantum Functional Materials Design and Application School of Physics and Electronic Engineering Jiangsu Normal University Xuzhou221116 China Institute of Physics Johannes Gutenberg University Mainz Mainz55099 Germany Peter Grünberg Institut Institute for Advanced Simulation Forschungszentrum Jülich and JARA Jülich52425 Germany

Mn3Sn has garnered significant attention due to its kagome lattice, 120◦ noncollinear antiferromagnetic order, and substantial anomalous Hall effect. In this study, we comprehensively explore intrinsic and extrinsic contributions to anomalous Hall, anomalous Nernst, and anomalous thermal Hall effects, employing first-principle calculations and group theory analysis. Comparative analysis between our theoretical results and available experimental data underscores the predominance of intrinsic mechanism in shaping anomalous transport properties at low temperatures. Specifically, Weyl fermions are identified as the primary contributors to intrinsic anomalous Hall conductivity. The significance of extrinsic mechanisms becomes evident at high temperatures, especially when the longitudinal charge conductivity falls into the dirty regime, where the side jump mechanism plays a vital role. Extrinsic contributions to anomalous transport properties are primarily influenced by the electronic states residing at the Fermi surfaces. Furthermore, anomalous transport properties exhibit periodic variations when subjected to spin rotations within the kagome plane, achievable by applying an external magnetic field. Our findings advance the understanding of anomalous transport phenomena in Mn3Sn and offer insights into potential applications of noncollinear antiferromagnetic materials in spintronics and spin caloritronics. Copyright © 2023, The Authors. All rights reserved.

关键词： Tin alloys

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Activation and Deactivation of Chirality Transfer in the Superbundles of Sequence-defined Stereoisomers

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Angewandte Chemie 2024年第4期137卷

作者： Zhihong Yu Rui Tan Xiaoxiao Cheng Wei Zhang Yong Wang Jiandong Zhang Nianchen Zhou Zhengbiao Zhang Xiulin Zhu State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China State Key Laboratory of Radiation Medicine and Protection Soochow University Suzhou 215123 China

Discrete oligomers can be used to precisely evaluate the structure–property relationship and enable unique chiroptical activities, however, the role of stereochemical sequences on chirality transfer is still unclear. Herein, we report the successful synthesis of a series of sequence-defined chiral azobenzene (Azo) oligomers via iterative stepwise chain growth strategy. Sequence-defined stereoisomers with one single chiral ( L or D ) stereocenter at the α-position, ω-position and middle- ( m −) position have completely different self-assembly dynamics. ω-positional stereocenter can effectively command all Azo building blocks to adopt a tilted π–π stacking along the helical superbundles, exhibiting the activation of chirality transfer. However, discrete oligomers with the stereocenter at other positions can only self-assemble into non-helical nanowires, accompanied by the deactivation of chirality *** supramolecular interactions, including the π–π interaction between Azo units, the intermolecular hydrogen bonding and steric hindrance, are intrinsic driving forces for these differentiations.

关键词： Precision synthesis Stereoisomer Chirality transfer Azobenzene Superbundles

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Rational design of a Negative Photochromic Spiropyran-Contained Fluorescent Polymeric Nanoprobe for Sulfur Dioxide Ratiometric Detection and in Vivo Imaging

SSRN

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SSRN 2022年

作者： Chen, Jian Li, Xiang Lin, Zhong Tian, Yong Zhang, Chonghua Zhang, Peisheng Zeng, Rongjin Qiao, Lei Key Laboratory of Theoretical Organic Chemistry and Functional Molecule of Ministry of Education Hunan Provincial Key Laboratory of Controllable Preparation and Functional Application of Fine Polymers Hunan Provincial Key Lab of Advanced Materials for New Energy Storage and Conversion Hunan Province College Key Laboratory of QSAR/QSPR School of Chemistry and Chemical Engineering Hunan University of Science and Technology Hunan Xiangtan411201 China Central Laboratory of the Affiliated Xuzhou Municipal Hospital of Xuzhou Medical University Xuzhou first People's Hospital Jiangsu Xuzhou221116 China Key Laboratory of Optic-Electric Sensing and Analytical Chemistry for Life Science MOE Shandong Key Laboratory of Biochemical Analysis College of Chemistry and Molecular Engineering Qingdao University of Science and Technology China

It is highly desirable to develop high-performance of ratiometric fluorescent probes for SO2 detection and realize their application in biological imaging and food detection. In this study, we reported the rational design of a novel negative photochromic spiropyran derivative as Spiro[azahomoadamantane-pyran] (MAHD-SP) with notable orange fluorescence in its stable ring-opened state without UV regulation. The unsaturated double bond of MAHD-SP can undergo Michael addition reaction of SO2 , which makes the obviously fluorescence quenching of MAHD-SP. Then, MAHD-SP, a fluorescent conjugated polymer PFO and a polymeric surfactant PEO113 - b -PS49 were used to construct a ratiometric fluorescent polymeric nanoprobe ( RFPN ) via co-precipitation method. The probe exhibited high sensitivity and selectivity toward ratiometric detection of SO2 in pure aqueous solutions. Moreover, RFPN was applied to quantitative analysis of SO2 in food and water samples. The good biocompatibility of RFPN can also be used to visualization of exogenous and endogenous SO2 generation in zebrafish model. © 2022, The Authors. All rights reserved.

关键词： Addition reactions

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Synthesis of curcumin polyprodrug via click chemistry and construction of dual-drug-loaded nano platform for highly efficient tumor treatment

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Chinese Chemical Letters 2025年第8期36卷

作者： Li, Haijiao Zhang, Mingzu He, Jinlin Liu, Jian Sun, Xingwei Ni, Peihong College of Chemistry Chemical Engineering and Materials Science State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis Soochow University Suzhou 215123 China Institute of Functional Nano and Soft Materials (FUNSOM) Soochow University Suzhou 215123 China Intervention Department The Second Affiliated Hospital of Soochow University Suzhou 215004 China

Micellar nanostructures formed by amphiphilic polymers are prone to dissociation when the in vivo environment changes. Polyprodrug micelles can cross-link with other hydrophobic drugs through non-covalent bonds, which has the advantage of fixed structure and avoids the use of chemical cross-linking agents. In this study, we prepared a polyprodrug with hydrophobic curcumin (CUR) and hydrophilic poly(ethylene glycol) (PEG) in the main chain through a click reaction between CUR derivatives containing azide groups and di-alkynly-capped PEG. Due to the presence of benzene rings in the structure of CUR, the polyprodrug can form non-covalent cross-linked nanoparticles (NCCL-CUR NPs) through hydrophobic and π-π stacking interaction. The structure, molecular weight, and self-assembly properties of the polyprodrug were characterized. The anti-cancer drug camptothecin (CPT) was encapsulated in the polyprodrug nanoparticles, producing dual-drug-loaded nanoparticles (abbreviated as CPT@NCCL-CUR NPs). The test results indicate that the NPs have reductive responsiveness and can release the original drugs CUR and CPT in phosphate buffer (PB) solution containing glutathione (GSH), while remaining stability in physiological environment. Cell and in vivo experiments further demonstrate that the dual-drug-loaded CPT@NCCL-CUR NPs can inhibit the growth of tumor through synergistic effects. This work provides a valuable approach for the preparation of amphiphilic polyprodrug with anti-tumor CUR as the backbone, and the stable dual-drug-loaded NPs containing both CUR and CPT through non-covalent cross-linking for synergistic therapy. © 2025

关键词： Camptothecin Click reaction Curcumin Non-covalent cross-linking Polyprodrug Stimuli responsiveness Synergistic therapy

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Photocontrolled Iodine-Mediated Reversible-Deactivation Radical Polymerization: Solution Polymerization of Methacrylates by Irradiation with NIR LED Light

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advanced Materials 2020年第10期59卷 3938-3944页

作者： Tian, Chun Wang, Peng Ni, Yuanyuan Zhang, Lifen Cheng, Zhenping Zhu, Xiulin State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou215123 China

Herein, near-infrared (NIR) photocontrolled iodidemediated reversible-deactivation radical polymerization (RDRP) of methacrylates, without an external photocatalyst, was developed using an alkyl iodide (e.g., 2-iodo-2-methylpropionitrile) as the initiator at room temperature. This example is the first use of a series of special solvents containing carbonyl groups (e.g., 1,3-dimethyl-2-imidazolidinone) as both solvent and catalyst for photocontrolled RDRP using long-wavelength (λmax=730 nm) irradiation. The polymerization system comprises monomer, alkyl iodide initiator, and solvent. Well-defined polymers were synthesized with excellent control over the molecular weights and molecular weight distributions (Mw/Mn © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

关键词： Solvents

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Photodynamic therapy-triggered on-demand drug release from ROS-responsive core-cross-linked micelles toward synergistic anti-cancer treatment

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Nano Research 2019年第5期12卷 999-1008页

作者： Yongjuan Li Jian Hu Xun Liu Yong Liu Shixian Lv Juanjuan Dang Yong Ji Jinlin He Lichen Yin Institute of Functional Nano and Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China College of Chemistry Chemical Engineering and Materials ScienceSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisJiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSoochow UniversitySuzhou 215123China Department of Biomedical Engineering University of Groningen and University Medical Center GroningenAntonius Deusinglaan 19713 AV Groningen The Netherlands Department of Cardiothoracic Surgery Wuxi Peoples Hospital Affiliated to Nanjing Medical UniversityWuxi 214023China

Polymeric micelles have demonstrated wide utility for chemodrug delivery,which however,still suffer from shortcomings such as undesired drug loading,disassembly upon dilution,pre-leakage of drug cargoes during systemic circulation,and lack of cancer-selective drug ***,a poly(ethylene glycol)(PEG)-polyphosphoester-based,reactive oxygen species (ROS)-responsive,core-cross-linked (CCL) micellar system was developed to encapsulate both chemodrug (doxorubicin,Dox) and photosensitizer (chlorin e6,Ce6).The hydrophobic core of the micelles was cross-linked via a thioketal (TK)-containing linker,which notably enhanced the drug loading and micelle *** tumor cells,far-red light irradiation of Ce6 generated ROS to cleave the TK linkers and disrupt the micelle *** such,micelles were destabilized and Dox release was promoted,which thereafter imparted synergistic anti-cancer effect with ROS-mediated photodynamic *** study provides an effective approach to realize the precise control over drug loading,formulation stability,and cancer-selective drug release using polymeric micelles,and would render promising utilities for the programmed anti-cancer combination therapy.

关键词： core-cross-linked micelles on-demand drug release photodynamic therapy reactive oxygen species (ROS) responsiveness synergistic an ti-cancer therapy

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